To develop air-operating conducting polymer (CP) actuators with enhanced performance, polymer electrolyte membranes with high ionic conductivity and mechanical endurance are necessary. Poly(ethylene oxide) oligomers penetrate into porous poly(vinylidene fluoride) membranes and sequentially undergo crosslinking to produce polymer electrolyte membranes. The properties of the electrolyte membranes are regulated by varying the degree of crosslinking. Polypyrrole layers are constructed on the surfaces of the membranes by chemical polymerization, creating CP actuators. CP actuators based on the resulting polymer electrolyte membranes operate properly in air and show highly enhanced performance such as a large displacement and long operation time. This approach, therefore, has great potential to extend the applications of CP actuators.